The ability to probe morphology and phase distribution in complex systems at multiple length scales unravels the interplay of nano‐ and micrometer‐scale factors at the origin of macroscopic behavior. While different electron‐ and X‐ray‐based imaging techniques can be combined with spectroscopy at high resolutions, owing to experimental time limitations the resulting fields of view are too small to be representative of a composite sample. Here a new X‐ray imaging set‐up is proposed, combining full‐field transmission X‐ray microscopy (TXM) with X‐ray absorption near‐edge structure (XANES) spectroscopy to follow two‐dimensional and three‐dimensional morphological and chemical changes in large volumes at high resolution (tens of nanometers). TXM XANES imaging offers chemical speciation at the nanoscale in thick samples (>20 µm) with minimal preparation requirements. Further, its high throughput allows the analysis of large areas (up to millimeters) in minutes to a few hours. Proof of concept is provided using battery electrodes, although its versatility will lead to impact in a number of diverse research fields. 相似文献
Successful X‐ray photon correlation spectroscopy studies often require that signals be optimized while minimizing power density in the sample to decrease radiation damage and, at free‐electron laser sources, thermal impact. This suggests exploration of scattering outside the Fraunhofer far‐field diffraction limit d2/λR, where d is the incident beam size, λ is the photon wavelength and R is the sample‐to‐detector distance. Here it is shown that, in an intermediate regime d2/λ > Rdξ/λ, where ξ is the structural correlation length in the material, the ensemble averages of the scattered intensity and of the structure factor are equal. Similarly, in the regime d2/λ > Rdξ(τ)/λ, where ξ(τ) is a time‐dependent dynamics length scale of interest, the ensemble‐averaged correlation functions g1(τ) and g2(τ) of the scattered electric field are also equal to their values in the far‐field limit. This broadens the parameter space for X‐ray photon correlation spectroscopy experiments, but detectors with smaller pixel size and variable focusing are required to more fully exploit the potential for such studies. 相似文献
Near‐field optical microscopy techniques provide information on the amplitude and phase of local fields in samples of interest in nanooptics. However, the information on the near field is typically obtained by converting it into propagating far fields where the signal is detected. This is the case, for instance, in polarization‐resolved scattering‐type scanning near‐field optical microscopy (s‐SNOM), where a sharp dielectric tip scatters the local near field off the antenna to the far field. Up to now, basic models have interpreted S‐ and P‐polarized maps obtained in s‐SNOM as directly proportional to the in‐plane ( or ) and out‐of‐plane () near‐field components of the antenna, respectively, at the position of the probing tip. Here, a novel model that includes the multiple‐scattering process of the probing tip and the nanoantenna is developed, with use of the reciprocity theorem of electromagnetism. This novel theoretical framework provides new insights into the interpretation of s‐SNOM near‐field maps: the model reveals that the fields detected by polarization‐resolved interferometric s‐SNOM do not correlate with a single component of the local near field, but rather with a complex combination of the different local near‐field components at each point (, and ). Furthermore, depending on the detection scheme (S‐ or P‐polarization), a different scaling of the scattered fields as a function of the local near‐field enhancement is obtained. The theoretical findings are corroborated by s‐SNOM experiments which map the near field of linear and gap plasmonic antennas. This new interpretation of nanoantenna s‐SNOM maps as a complex‐valued combination of vectorial local near fields is crucial to correctly understand scattering‐type near‐field microscopy measurements as well as to interpret the signals obtained in field‐enhanced spectroscopy.
X‐ray absorption near‐edge structure (XANES) and X‐ray photoelectron spectroscopy (XPS) of Nd‐doped phosphate glasses have been studied before and after gamma irradiation. The intensity and the location of the white line peak of the L3‐edge XANES of Nd are found to be dependent on the ratio O/Nd in the glass matrix. Gamma irradiation changes the elemental concentration of atoms in the glass matrix, which affects the peak intensity of the white line due to changes in the covalence of the chemical bonds with Nd atoms in the glass (structural changes). Sharpening of the Nd 3d5/2 peak profile in XPS spectra indicates a deficiency of oxygen in the glasses after gamma irradiation, which is supported by energy‐dispersive X‐ray spectroscopy measurements. The ratio of non‐bridging oxygen to total oxygen in the glass after gamma radiation has been found to be correlated to the concentration of defects in the glass samples, which are responsible for its radiation resistance as well as for its coloration. 相似文献
A VUV absorption spectroscopy facility designed for ultra‐high spectral resolution is in operation as a dedicated branch on the DESIRS beamline at Synchrotron SOLEIL. This branch includes a unique VUV Fourier transform spectrometer (FTS) and a dedicated versatile gas sample chamber. The FTS instrument can cover a large UV–VUV spectral range from 4 to 30 eV, with an ultimate line width of 0.08 cm?1 on a large spectral window, ΔE/E = 7%, over which all spectral features can be acquired in a multiplex way. The performance can be considered to be a middle ground between broadband moderate‐resolution spectrometers based on gratings and ultra‐high‐spectral‐resolution VUV tunable‐laser‐based techniques over very narrow spectral windows. The various available gaseous‐sample‐handling setups, which function over a wide range of pressures and temperatures, and the acquisition methodology are described. A selection of experimental results illustrates the performance and limitations of the FTS‐based facility. 相似文献
X‐Treme is a soft X‐ray beamline recently built in the Swiss Light Source at the Paul Scherrer Institut in collaboration with École Polytechnique Fédérale de Lausanne. The beamline is dedicated to polarization‐dependent X‐ray absorption spectroscopy at high magnetic fields and low temperature. The source is an elliptically polarizing undulator. The end‐station has a superconducting 7 T–2 T vector magnet, with sample temperature down to 2 K and is equipped with an in situ sample preparation system for surface science. The beamline commissioning measurements, which show a resolving power of 8000 and a maximum flux at the sample of 4.7 × 1012 photons s?1, are presented. Scientific examples showing X‐ray magnetic circular and X‐ray magnetic linear dichroism measurements are also presented. 相似文献
We use moving‐window two‐dimensional correlation spectroscopy (MW‐2DCOS) for phase‐specific Raman analysis of the n‐alkane (C21H44) during melting from the crystalline solid phase to the intermediate rotator phase and to the amorphous molten phase. In MW‐2DCOS, individual peak‐to‐peak correlation analysis within a small subset of spectra provides both temperature‐resolved and spectrally disentangled Raman assignments conducive to understanding phase‐specific molecular interactions and chain configurations. We demonstrate that autocorrelation MW‐2DCOS can determine the phase transition temperatures with a higher resolving power than commonly used analysis methods including individual peak intensity analysis or principal component analysis. Besides the enhanced temperature resolving power, we demonstrate that asynchronous 2DCOS near the orthorhombic‐to‐rotator transition temperature can spectrally resolve the two overlapping peaks embedded in the Raman CH2 twisting band in the orthorhombic phase, which had been only predicted but not observed because of thermal broadening near the melting temperature. Published 2016. This article is a U.S. Government work and is in the public domain in the USA. 相似文献
With the modern development of infrared laser sources such as broadly tunable quantum cascade lasers and frequency combs, applications of infrared laser spectroscopy are expected to become widespread. Consequently, convenient infrared detectors are needed, having properties such as fast response, high efficiency, and room‐temperature operation. This work investigated conditions to achieve near‐room‐temperature photon‐noise‐limited performance of quantum well infrared photodetectors (QWIPs), in particular the laser power requirement. Both model simulation and experimental verification were carried out. At 300 K, it is shown that the ideal performance can be reached for typical QWIP designs up to a detection wavelength of 10 µm. At 250 K, which is easily reachable with a thermoelectric Peltier cooler, the ideal performance can be reached up to 12 µm. QWIPs are therefore suitable for detection and sensing applications with devices operating up to or near room temperature. 相似文献